Understanding and manipulating the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity.Herein,we present a synthesis of NiSe_(2)-Ce_(2)(CO_(3))_(2)O hetero...Understanding and manipulating the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity.Herein,we present a synthesis of NiSe_(2)-Ce_(2)(CO_(3))_(2)O heterostructure and demonstrate the efficacy of interfacial Ce_(2)(CO_(3))2O in promoting the formation of catalytically active centers to improve oxygen evolution activity.In-situ Raman spectroscopy shows that incorporation of Ce_(2)(CO_(3))2O into NiSe_(2) causes a cathodic shift of the Ni^(2+)→Ni~(3+) transition potential.Operando electrochemical impedance spectroscopy reveals that strong electronic coupling at heterogeneous interface accelerates charge transfer process.Furthermore,density functional theory calculations suggest that actual catalytic active species of NiOOH transformed from NiSe_(2),which is coupled with Ce_(2)(CO_(3))_(2)O,can optimize electronic structure and decrease the free energy barriers toward fast oxygen evolution reaction(OER) kinetics.Consequently,the resultant NiSe_(2)-Ce_(2)(CO_(3))_(2)O electrode exhibits remarkable electrocatalytic performance with low overpotentials(268/304 mV@50/100 mA cm^(-2)) and excellent stability(50 mA cm^(-2) for 120 h) in the alkaline electrolyte.This work emphasizes the significance of modulating the dynamic changes in developing efficient electrocatalyst.展开更多
基金financially National Natural Science Foundation of China (52363028, 21965005)Volkswagen Foundation (Freigeist Fellowship 89592)+2 种基金Natural Science Foundation of Guangxi Province (2021GXNSFAA076001)Guangxi Technology Base and Talent Subject (GUIKE AD23023004, GUIKE AD20297039)Innovation Project of Guangxi Graduate Education (Nos. YCSW2024219, YCBZ2024082)。
文摘Understanding and manipulating the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity.Herein,we present a synthesis of NiSe_(2)-Ce_(2)(CO_(3))_(2)O heterostructure and demonstrate the efficacy of interfacial Ce_(2)(CO_(3))2O in promoting the formation of catalytically active centers to improve oxygen evolution activity.In-situ Raman spectroscopy shows that incorporation of Ce_(2)(CO_(3))2O into NiSe_(2) causes a cathodic shift of the Ni^(2+)→Ni~(3+) transition potential.Operando electrochemical impedance spectroscopy reveals that strong electronic coupling at heterogeneous interface accelerates charge transfer process.Furthermore,density functional theory calculations suggest that actual catalytic active species of NiOOH transformed from NiSe_(2),which is coupled with Ce_(2)(CO_(3))_(2)O,can optimize electronic structure and decrease the free energy barriers toward fast oxygen evolution reaction(OER) kinetics.Consequently,the resultant NiSe_(2)-Ce_(2)(CO_(3))_(2)O electrode exhibits remarkable electrocatalytic performance with low overpotentials(268/304 mV@50/100 mA cm^(-2)) and excellent stability(50 mA cm^(-2) for 120 h) in the alkaline electrolyte.This work emphasizes the significance of modulating the dynamic changes in developing efficient electrocatalyst.
